Simplified bond-hyperpolarizability model of second harmonic generation: Application to Si-dielectric interfaces

Sensitivity of second harmonic generation to space charge effects at Si(111 )/electrolyte and Si(111 )/SiO~electrolyte trolyte interfaces

The potential dependence in the surlace second hannonic response from hydrogen terminated n-Si(111) i(l l and oxidized n-Si(1l1) ll surfaces has been examined in aqueous NH4F and H2S04 4 solutions. The relative phase of the nonlinear response as measured by rotational anisotropy experiments is found to be highly sensitive to the presence of the oxide and the field applied across Si(ll I)/mdde/e...

Polarity of Liquid Interfaces by Second Harmonic Generation Spectroscopy

A spectroscopic method, based on the interface selectivity of second-harmonic generation, is used to obtain the polarity of liquid interfaces. In this paper the second-harmonic measurement of the spectrum of the polarity indicator molecule N,N′-diethyl-p-nitroaniline (DEPNA) at the air/water interface demonstrates the method. Two different approaches are used to measure the intramolecular charg...

electric-field-induced second harmonic generation ~ESHG! vibrational second hyperpolarizability of CF4. With the exception of the small ESHG vibrational second hyperpolarizability the infinite optical frequency method

The frequency-dependent vibrational second hyperpolarizability of CH42nFn molecules with n 50 – 4 has been computed for the most common nonlinear optical ~NLO! processes by adopting the perturbation approach due to Bishop and Kirtman @J. Chem. Phys. 95, 2646 ~1991!#. These calculations have been performed by using the Sadlej atomic basis set with the Hartree-Fock technique as well as with the M...

Optimization of the molecular hyperpolarizability for second harmonic generation in chiral media

Molecular properties leading to second harmonic generation in chiral media in the electric dipole approximation for the cases of axial and biaxial symmetry are described. The components of the hyperpolarizability tensor that transform like a second-rank pseudotensor (L ˆ 2) and a third-rank tensor (L ˆ 3) contribute. The sum-over-states quantum formula for the hyperpolarizability is used to ill...

Magnetization-induced-second -harmonic generation from surfaces and interfaces